Unlike the facile modulation of surface structure through protecting ligands,the core shielded by outer shell of silver nanoclusters is still hard to be controlled.Ligand effects may seep into the incipient growth of ...Unlike the facile modulation of surface structure through protecting ligands,the core shielded by outer shell of silver nanoclusters is still hard to be controlled.Ligand effects may seep into the incipient growth of silver core.However,the comparable cases to validate such hypothesis are currently lacking.Herein,we shed light on two core-shell silver nanoclusters,Ag_(7)S_(6)@Ag_(48)(SD/Ag55b,SD=SunDi)and Ag_(6)S_(6)@Ag_(48)(SD/Ag54b),differing in only one silver atom in the core which varies from a pentagon-bipyramidal Ag_(7)to an octahedral Ag_(6)while keeping the Ag_(48)shielding shell almost the same.Although no direct bonding between alkynes and silver core is observed in them,we propose that the ligand effect still exerts profound influences on the size and geometry of silver core.The solution behaviours and complete ligand-exchange reaction of SD/Ag55b in CH_(2)Cl_(2)are investigated using electrospray ionization mass spectrometry.Due to more and stronger argentophilic interactions,SD/Ag55b exhibits room-temperature phosphorescence with a 40 nm red-shift compared to that of SD/Ag54b in CH_(2)Cl_(2).This work not only presents effective fabrication of silver nanoclusters via synergism of dithiophosphate and alkyne ligands,but also provides us a pair of comparable examples to understand substitution group effect of protecting ligand on the core structures and properties.展开更多
A multi-scale hardware and software architecture implementing the EMMS （energy-minimization multi-scale） paradigm is proven to be effective in the simulation of a two-dimensional gas-solid suspension. General purpos...A multi-scale hardware and software architecture implementing the EMMS （energy-minimization multi-scale） paradigm is proven to be effective in the simulation of a two-dimensional gas-solid suspension. General purpose CPUs are employed for macro-scale control and optimization, and many integrated cores （MlCs） operating in multiple-instruction multiple-data mode are used for a molecular dynamics simulation of the solid particles at the meso-scale. Many cores operating in single-instruction multiple- data mode, such as general purpose graphics processing units （GPGPUs）, are employed for direct numerical simulation of the fluid flow at the micro-scale using the lattice Boltzmann method. This architecture is also expected to be efficient for the multi-scale simulation of other comolex systems.展开更多
基金supported by the National Natural Science Foundation of China(91961105,21822107)the Fok Ying Tong Education Foundation(171009)+3 种基金the Natural Science Foundation of Shandong Province(ZR2019ZD45,ZR2020ZD35,JQ201803,ZR2017MB061)the Taishan Scholar Project of Shandong Province of China(tsqn201812003,ts20190908)the Qilu Youth Scholar Funding of Shandong UniversityProject for Scientific Research Innovation Team of Young Scholar in Colleges and Universities of Shandong Province(2019KJC028)。
文摘Unlike the facile modulation of surface structure through protecting ligands,the core shielded by outer shell of silver nanoclusters is still hard to be controlled.Ligand effects may seep into the incipient growth of silver core.However,the comparable cases to validate such hypothesis are currently lacking.Herein,we shed light on two core-shell silver nanoclusters,Ag_(7)S_(6)@Ag_(48)(SD/Ag55b,SD=SunDi)and Ag_(6)S_(6)@Ag_(48)(SD/Ag54b),differing in only one silver atom in the core which varies from a pentagon-bipyramidal Ag_(7)to an octahedral Ag_(6)while keeping the Ag_(48)shielding shell almost the same.Although no direct bonding between alkynes and silver core is observed in them,we propose that the ligand effect still exerts profound influences on the size and geometry of silver core.The solution behaviours and complete ligand-exchange reaction of SD/Ag55b in CH_(2)Cl_(2)are investigated using electrospray ionization mass spectrometry.Due to more and stronger argentophilic interactions,SD/Ag55b exhibits room-temperature phosphorescence with a 40 nm red-shift compared to that of SD/Ag54b in CH_(2)Cl_(2).This work not only presents effective fabrication of silver nanoclusters via synergism of dithiophosphate and alkyne ligands,but also provides us a pair of comparable examples to understand substitution group effect of protecting ligand on the core structures and properties.
基金supported by the National Science Foundation for Distinguished Young Scholars of China under Grant No.21225628the Science Fund for Creative Research Groups of the National Natural Science Foundation of China under Grant No.20821092+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences under Grant No.XDA07080100the National Natural Science Foundation of China under Grant No. 21206167
文摘A multi-scale hardware and software architecture implementing the EMMS （energy-minimization multi-scale） paradigm is proven to be effective in the simulation of a two-dimensional gas-solid suspension. General purpose CPUs are employed for macro-scale control and optimization, and many integrated cores （MlCs） operating in multiple-instruction multiple-data mode are used for a molecular dynamics simulation of the solid particles at the meso-scale. Many cores operating in single-instruction multiple- data mode, such as general purpose graphics processing units （GPGPUs）, are employed for direct numerical simulation of the fluid flow at the micro-scale using the lattice Boltzmann method. This architecture is also expected to be efficient for the multi-scale simulation of other comolex systems.
